Tuning strategy for Curie-temperature enhancement in the van der Waals magnet Mn_1+xSb_2−xTe₄

The van-der-Waals antiferromagnetic topological insulator MnBi2Te4 is one of the few materials that realize the sought-after quantum anomalous Hall (QAH) state and quantized surface charge transport. To assess the relevance of its isostructural analog MnSb2Te4 as a potential QAH candidate, the roles of Mn/Sb site mixing and cationic vacancies need to be clarified. Recent findings have shown that non-stoichiometry in Mn1±xSb2∓xTe4 is an efficient tuning knob to achieve a net spin-polarized state and to raise the magnetic ordering temperature well above that of MnBi2Te4. Here, we report the crystal structure, the bulk and the surface magnetism of two new Mn1+xSb2−xTe4 samples: Mn1.08Sb1.92Te4(x ≈ 0.1) with TC = 44 K, and Mn2.01Sb1.19Te4(x ≈ 1.0) with the record TC = 58 K. We quantify the site mixing comprehensively by combining various structural probes on powders and single crystals, and then employ bulk, local (electron spin resonance), and spectroscopic (x-ray magnetic circular dichroism) probes to connect these insights to the magnetism of these materials. We demonstrate that Mn over-stoichiometry up to x = 1.0, in combination with a particular Mn/Sb intermixing pattern and the increasingly three-dimensional character of the magnetic order, push the TC upwards. The tendency towards more robust ferromagnetism mediated by stronger interlayer exchange in Mn1+xSb2−xTe4 upon increasing x is confirmed by bulk magnetometry and by a series of density-functional-theory calculations of model structures with varying intermixing.</p

Two-dimensional ferromagnetic extension of a topological insulator

Inducing a magnetic gap at the Dirac point of the topological surface state (TSS) in a three-dimensional (3D) topological insulator (TI) is a route to dissipationless charge and spin currents. Ideally, magnetic order is present only at the surface, as through proximity of a ferromagnetic (FM) layer. However, experimental evidence of such a proximity-induced Dirac mass gap is missing, likely due to an insufficient overlap of TSS and the FM subsystem. Here, we take a different approach, namely ferromagnetic extension (FME), using a thin film of the 3D TI Bi2Te3, interfaced with a monolayer of the lattice-matched van der Waals ferromagnet MnBi2Te4. Robust 2D ferromagnetism with out-of-plane anisotropy and a critical temperature of Tc ≈ 15 K is demonstrated by x-ray magnetic dichroism and electrical transport measurements. Using angle-resolved photoelectron spectroscopy, we observe the opening of a sizable magnetic gap in the 2D FM phase, while the surface remains gapless in the paramagnetic phase above Tc. Ferromagnetic extension paves the way to explore the interplay of strictly 2D magnetism and topological surface states, providing perspectives for realizing robust quantum anomalous Hall and chiral Majorana states.</p

Two-dimensional ferromagnetic extension of a topological insulator

Inducing a magnetic gap at the Dirac point of the topological surface state (TSS) in a 3D topological insulator (TI) is a route to dissipationless charge and spin currents. Ideally, magnetic order is present only at the surface and not in the bulk, e.g. through proximity of a ferromagnetic (FM) layer. However, such a proximity-induced Dirac mass gap has not been observed, likely due to insufficient overlap of TSS and the FM subsystem. Here, we take a different approach, namely FM extension, using a thin film of the 3D TI Bi$_2$Te$_3$, interfaced with a monolayer of the lattice-matched van der Waals ferromagnet MnBi$_2$Te$_4$. Robust 2D ferromagnetism with out-of-plane anisotropy and a critical temperature of $\text{T}_\text{c}\approx$~15 K is demonstrated by X-ray magnetic dichroism and electrical transport measurements. Using angle-resolved photoelectron spectroscopy, we observe the opening of a sizable magnetic gap in the 2D FM phase, while the surface remains gapless in the paramagnetic phase above T$_c$. This sizable gap indicates a relocation of the TSS to the FM ordered Mn moments near the surface, which leads to a large mutual overlap.Comment: 6 pages, 3 figure

Two-dimensional ferromagnetic extension of a topological insulator

Inducing a magnetic gap at the Dirac point of the topological surface state (TSS) in a three-dimensional (3D) topological insulator (TI) is a route to dissipationless charge and spin currents. Ideally, magnetic order is present only at the surface, as through proximity of a ferromagnetic (FM) layer. However, experimental evidence of such a proximity-induced Dirac mass gap is missing, likely due to an insufficient overlap of TSS and the FM subsystem. Here, we take a different approach, namely ferromagnetic extension (FME), using a thin film of the 3D TI Bi2Te3, interfaced with a monolayer of the lattice-matched van der Waals ferromagnet MnBi2Te4. Robust 2D ferromagnetism with out-of-plane anisotropy and a critical temperature of Tc≈15 K is demonstrated by x-ray magnetic dichroism and electrical transport measurements. Using angle-resolved photoelectron spectroscopy, we observe the opening of a sizable magnetic gap in the 2D FM phase, while the surface remains gapless in the paramagnetic phase above Tc. Ferromagnetic extension paves the way to explore the interplay of strictly 2D magnetism and topological surface states, providing perspectives for realizing robust quantum anomalous Hall and chiral Majorana states

Author Correction: Non-local effect of impurity states on the exchange coupling mechanism in magnetic topological insulators

A Correction to this paper has been published: https://doi.org/10.1038/s41535-021-00314-

Magnetic field dependence of the copper charge density wave order in a YBa2Cu3O7 Nd0.65 Ca0.7Sr0.3 0.35MnO3 superlattice

For a YBa2Cu3O7 Nd0.65 Ca0.7Sr0.3 0.35MnO3 YBCO NCSMO superlattice, we studied with resonant elastic x ray scattering REXS at the Cu L3 edge how the copper sublattice charge density wave Cu CDW order in YBCO is affected by a large magnetic field up to 6.9 T that weakens the CE type antiferromagnetic AF and the charge orbital Mn CO orders of the manganite in favor of a ferromagnetic state. While a field of only 2 T induces a strong ferromagnetic moment in the manganite, we find that the Bragg peak of the Cu CDW hardly changes up to 6 T. Moreover, as the magnetic field is further increased to 6.9 T, the Cu CDW Bragg peak gets suddenly enhanced and broadened, whereas the ferromagnetic moment of the manganite is already saturated. The observed uncorrelated magnetic field dependence of the charge orders in the cuprate and manganite layers suggests that these orders are not directly coupled across the interface. We rather interpret our data in terms of an indirect coupling via the domain boundaries of the Mn CO and the related disorder and lattice strain. This interpretation is supported by additional studies of the magnetoelectric response, which provide evidence for a crossover in the dynamics of the Mn CO in the range between 6 and 7 T, from a low field state with pinned domains to a high field state with more mobile and flexible domain boundaries. We attribute the concomitant enhancement and broadening of the Cu CDW Bragg peak to this crossove

Incorporation of Europium in Bi₂Te₃ Topological Insulator Epitaxial Films

In the field of topological materials, the interaction between band topology and magnetism remains a current frontier for the advancement of new topological states and spintronic functionalities. Doping with rare-earth elements with large magnetic moments is a current approach to exploit the phenomenology of such interaction. However, dopant solubility into the main matrix plays a major role. In this sense, the present work is focused on elucidating how Eu incorporates into Bi2Te3 lattice as a function of doping. This work reports a systematic investigation of the structural and electronic properties of bismuth telluride epitaxial layers doped with Eu. Bi2Te3 films were grown by molecular beam epitaxy on (111) BaF2 substrates with nominal Eu doping ranging from 0% up to 9%. X-ray diffraction analysis and scanning transmission electron microscopy reveal that Eu atoms enter substitutionally on Bi sites up to 4% of Eu doping. In contrast, the 9% Eu-doped sample contains epitaxially oriented nanoclusters of EuTe. X-ray photoelectron and absorption spectroscopies show that Eu atoms enter the Bi2Te3 crystal matrix in the divalent Eu2+ state for all Eu concentrations. Angle-resolved photoemission experiments indicate that the topological surface state is preserved in the presence of the local magnetic moments introduced by the Eu impurities

Incorporation of Europium in Bi2Te3 Topological Insulator Epitaxial Films

In the field of topological materials, the interaction between band topology and magnetism remains a current frontier for the advancement of new topological states and spintronic functionalities. Doping with rare-earth elements with large magnetic moments is a current approach to exploit the phenomenology of such interaction. However, dopant solubility into the main matrix plays a major role. In this sense, the present work is focused on elucidating how Eu incorporates into Bi2Te3 lattice as a function of doping. This work reports a systematic investigation of the structural and electronic properties of bismuth telluride epitaxial layers doped with Eu. Bi2Te3 films were grown by molecular beam epitaxy on (111) BaF2 substrates with nominal Eu doping ranging from 0% up to 9%. X-ray diffraction analysis and scanning transmission electron microscopy reveal that Eu atoms enter substitutionally on Bi sites up to 4% of Eu doping. In contrast, the 9% Eu-doped sample contains epitaxially oriented nanoclusters of EuTe. X-ray photoelectron and absorption spectroscopies show that Eu atoms enter the Bi2Te3 crystal matrix in the divalent Eu2+ state for all Eu concentrations. Angle-resolved photoemission experiments indicate that the topological surface state is preserved in the presence of the local magnetic moments introduced by the Eu impurities